It is still a great challenge to develop efficient semiconductive photocatalysts responding to visible light radiation. We show an efficient ZnIn2S4/UiO-66 hybrid photocatalysts with flowerlike 3D microspheres synthesized via a facile solvothermal method. A 20 wt.% UiO-66 emersion raises the Cr(VI) reduction rate up to 99% and higher after 60 min visible light irradiation. The substantial enhancement of photocatalytic and photoelectronchemical activity of pure ZnIn2S4 by UiO-66 addition is attributed to the ZnIn2S4/UiO-66 interfacial charge transferring and more active sites for pollute adsorption.